Visible-light harvesting pyrene-based MOFs as efficient ROS generators.
Yingmu ZhangJiandong PangJia-Luo LiXinyu YangMingbao FengPeiyu CaiHong-Cai ZhouPublished in: Chemical science (2019)
The utilization of reactive oxygen species (ROS) in organic transformations is of great interest due to their superior oxidative abilities under mild conditions. Recently, metal-organic frameworks (MOFs) have been developed as photosensitizers to transfer molecular oxygen to ROS for photochemical synthesis. However, visible-light responsive MOFs for oxygen activation remains scarce. Now we design and synthesize two porous MOFs, namely, PCN-822(M) (M = Zr, Hf), which are constructed by a 4,5,9,10-(K-region) substituted pyrene-based ligand, 4,4',4'',4'''-((2,7-di-tert-butylpyrene-4,5,9,10-tetrayl)tetrakis(ethyne-2,1-diyl))-tetrabenzoate (BPETB4-). With the extended π-conjugated pyrene moieties isolated on the struts, the derived MOFs are highly responsive to visible light, possessing a broad-band adsorption from 225-650 nm. As a result, the MOFs can be applied as efficient ROS generators under visible-light irradiation, and the hafnium-based MOF, PCN-822(Hf), can promote the oxidation of amines to imines by activating molecular oxygen via synergistic photo-induced energy and charge transfer.
Keyphrases
- visible light
- metal organic framework
- reactive oxygen species
- cell death
- dna damage
- photodynamic therapy
- cancer therapy
- single molecule
- escherichia coli
- heart failure
- wastewater treatment
- computed tomography
- molecular docking
- oxidative stress
- acute heart failure
- nitric oxide
- pseudomonas aeruginosa
- pet imaging
- cystic fibrosis
- atrial fibrillation
- high glucose
- biofilm formation
- staphylococcus aureus
- molecular dynamics simulations
- stress induced
- hydrogen peroxide
- light emitting